10.1021/ja304049x.s001
Qing Guo
Qing
Guo
Chenbiao Xu
Chenbiao
Xu
Zefeng Ren
Zefeng
Ren
Wenshao Yang
Wenshao
Yang
Zhibo Ma
Zhibo
Ma
Dongxu Dai
Dongxu
Dai
Hongjun Fan
Hongjun
Fan
Timothy K. Minton
Timothy K.
Minton
Xueming Yang
Xueming
Yang
Stepwise Photocatalytic
Dissociation of Methanol and
Water on TiO<sub>2</sub>(110)
American Chemical Society
2012
BBO
calculation
photocatalytic methanol dissociation
Stepwise Photocatalytic Dissociation
Theoretical
TiO
H 2O photocatalytic dissociation
CD 2O
Ti 5c sites
recombination
photocatalytic water splitting
CD 3OH
H 2O photocatalysis
2012-08-15 00:00:00
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Stepwise_Photocatalytic_Dissociation_of_Methanol_and_Water_on_TiO_sub_2_sub_110_/2496193
We have investigated the photocatalysis of partially
deuterated
methanol (CD<sub>3</sub>OH) and H<sub>2</sub>O on TiO<sub>2</sub>(110)
at 400 nm using a newly developed photocatalysis apparatus in combination
with theoretical calculations. Photocatalyzed products, CD<sub>2</sub>O on Ti<sub>5c</sub> sites, and H and D atoms on bridge-bonded oxygen
(BBO) sites from CD<sub>3</sub>OH have been clearly detected, while
no evidence of H<sub>2</sub>O photocatalysis was found. The experimental
results show that dissociation of CD<sub>3</sub>OH on TiO<sub>2</sub>(110) occurs in a stepwise manner in which the O–H dissociation
proceeds first and is then followed by C–D dissociation. Theoretical
calculations indicate that the high reverse barrier to C–D
recombination and the facile desorption of CD<sub>2</sub>O make photocatalytic
methanol dissociation on TiO<sub>2</sub>(110) proceed efficiently.
Theoretical results also reveal that the reverse reactions, i.e, O–H
recombination after H<sub>2</sub>O photocatalytic dissociation on
TiO<sub>2</sub>(110), may occur easily, thus inhibiting efficient
photocatalytic water splitting.